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公开(公告)号:US20230114770A1
公开(公告)日:2023-04-13
申请号:US17914395
申请日:2021-03-26
Applicant: BASF SE
Inventor: Andrey KARPOV , Christian WALSDORFF , Thorsten JOHANN , Christian ALMER , Daniela RIECK , Christian BARTOSCH , Mauricio GROBYS , Tobias WEINLAND , Holger BORCHERT
IPC: B01J23/68 , B01J37/02 , B01J37/14 , B01J37/16 , C07D301/10
Abstract: A process for producing a silver-based epoxidation catalyst, comprising i) impregnating a particulate porous refractory support with a first aqueous silver impregnation solution comprising silver ions and an aminic complexing agent selected from amines, alkanolamines and amino acids; ii) converting at least part of the silver ions impregnated on the refractory support to metallic silver by heating while directing a stream of a first gas over the impregnated refractory support to obtain an intermediate catalyst, wherein the first gas comprises at least 5 vol.-% oxygen; iii) impregnating the intermediate catalyst with a second aqueous silver impregnation solution comprising silver ions, an aminic complexing agent selected from amines, alkanolamines and amino acids, and one or more transition metal promoters, in particular rhenium; and iv) converting at least part of the silver ions impregnated on the intermediate catalyst to metallic silver by heating while directing a stream of a second gas over the impregnated intermediate catalyst to obtain the epoxidation catalyst, wherein the second gas comprises at most 2.0 vol.-% oxygen, wherein the impregnated refractory support and the impregnated intermediate catalyst are each heated to a temperature of 200 to 800° C. The process of the invention surprisingly allows for obtaining a catalyst with high selectivity in a cost-efficient manner. The invention also relates to a silver-based epoxidation catalyst obtainable by such a process, and to a process for producing an alkylene oxide by gas-phase oxidation of an alkylene, comprising reacting an alkylene and oxygen in the presence of a silver-based epoxidation catalyst obtainable by the above process.
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公开(公告)号:US20210387958A1
公开(公告)日:2021-12-16
申请号:US17285780
申请日:2019-09-19
Applicant: BASF SE
Inventor: Andrey KARPOV , Marco Oskar KENNEMA , Nicolas DUYCKAERTS , Christian WALSDORFF , Christian BARTOSCH , Juergen ZUEHLKE , Miguel Angel ROMERO VALLE
Abstract: A process for producing ethylene oxide by gas-phase oxidation of ethylene, comprising: directing a feed comprising gaseous ethylene and gaseous oxygen through a packing of individual shaped catalyst bodies, under conditions conducive to obtain a reaction mixture containing at least 2.7 vol.-% of ethylene oxide, wherein each shaped catalyst body comprises silver deposited on a refractory support and is characterized by a content of at least 20 wt.-% of silver, relative to the total weight of the shaped catalyst body; a BET surface area in the range of 1.6 to 3.0 m2/g; a first face side surface, a second face side surface and a circumferential surface with a plurality of passageways extending from the first face side surface to the second face side surface; and a uniform multilobed cross-section; and a longest direct diffusion pathway d, with 2d being in the range of 0.7 to 2.4 mm, wherein the longest diffusion pathway d is defined as the shortest distance from the geometric surface of the shaped catalyst body to a point inside the structure of the shaped catalyst body for which point the shortest distance is the largest among all points. The process allows for increased activity and/or stability of the catalyst while maintaining or increasing selectivity at high productivity.
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公开(公告)号:US20160332152A1
公开(公告)日:2016-11-17
申请号:US14907714
申请日:2014-07-16
Applicant: BASF SE , DOW GLOBAL TECHNOLOGIES LLC
Inventor: Andrei-Nicolae PARVULESCU , Ulrich MUELLER , Joaquim Henrique TELES , Bianca SEELIG , Philip KAMPE , Markus WEBER , Peter RESCH , Christian BARTOSCH , Dominic RIEDEL , Daniel URBANCZYK , Alexander SCHROEDER , Ulrike WEGERLE
IPC: B01J29/90 , B01J37/02 , B01J37/00 , C07D301/12 , B01J37/30 , B01J38/48 , B01J38/06 , B01J38/02 , B01J29/70 , B01J37/08
CPC classification number: B01J29/90 , B01J29/7088 , B01J29/89 , B01J35/00 , B01J37/0009 , B01J37/0045 , B01J37/0201 , B01J37/0203 , B01J37/06 , B01J37/08 , B01J37/10 , B01J37/30 , B01J38/02 , B01J38/06 , B01J38/48 , B01J2229/183 , B01J2229/186 , B01J2229/42 , C07D301/12 , C07D303/04 , Y02P20/584
Abstract: The present invention relates to a process for the regeneration of a catalyst comprising a titanium-containing zeolite, said catalyst having been used in a process for the preparation of an olefin oxide and having phosphate deposited thereon, said process for the regeneration comprising the steps: (a) separating the reaction mixture from the catalyst, (b) washing the catalyst obtained from (a) with liquid aqueous system; (c) optionally drying the catalyst obtained from (b) in a gas stream comprising an inert gas at a temperature of less than 300° C.; (d) calcining the catalyst obtained from (c) in a gas stream comprising oxygen at a temperature of at least 300° C.
Abstract translation: 本发明涉及一种用于再生包含含钛沸石的催化剂的方法,所述催化剂已用于制备烯烃氧化物并沉积有磷酸盐的方法中,所述再生方法包括以下步骤: (a)将反应混合物与催化剂分离,(b)用液体水系洗涤由(a)获得的催化剂; (c)任选地在低于300℃的温度下将包含惰性气体的气流中的(b)得到的催化剂干燥; (d)在至少300℃的温度下,将由(c)得到的催化剂在包含氧的气流中煅烧
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公开(公告)号:US20160176834A1
公开(公告)日:2016-06-23
申请号:US14907998
申请日:2014-07-16
Applicant: BASF SE , DOW GLOBAL TECHNOLOGIES LLC
Inventor: Joaquim Henrique TELES , Bianca SEELIG , Dominic RIEDEL , Philip KAMPE , Daniel URBANCZYK , Markus WEBER , Ulrich MUELLER , Andrei-Nicolae PARVULESCU , Kai GUMLICH , Peter BASSLER , Christian BARTOSCH , Richard JACUBINAS , Meinolf WEIDENBACH , Werner WITZL
IPC: C07D301/12 , B01J27/188 , B01J27/18 , B01J29/70
CPC classification number: C07D301/12 , B01J27/18 , B01J27/188 , B01J29/7038 , B01J29/7088 , B01J35/002 , B01J35/1019 , B01J2229/186 , Y02P20/52
Abstract: A continuous process for the preparation of propylene oxide, comprising (i) providing a liquid feed stream comprising propene, hydrogen peroxide, acetonitrile, water, optionally propane, and at least one dissolved potassium salt of a phosphorus oxyacid wherein the molar ratio of potassium relative to phosphorus in the at least one potassium salt of a phosphorus oxyacid is in the range of from 0.6 to 1.4; (ii) passing the liquid feed stream provided in (i) into an epoxidation reactor comprising a catalyst comprising a titanium zeolite of structure type MVVW comprising zinc, and subjecting the liquid feed stream to epoxidation reaction conditions in the epoxidation reactor, obtaining a reaction mixture comprising propylene oxide, acetonitrile, water, the at least one dissolved potassium salt of a phosphorus oxyacid, optionally propene, and optionally propane; (iii) removing an effluent stream from the epoxidation reactor, the effluent stream comprising propylene oxide, acetonitrile, water, at least a portion of the at least one dissolved potassium salt of a phosphorus oxyacid, optionally propene, and optionally propane.
Abstract translation: 一种用于制备环氧丙烷的连续方法,包括(i)提供包含丙烯,过氧化氢,乙腈,水,任选的丙烷和至少一种溶解的含磷酸钾的液体进料流,其中钾相对的摩尔比 在磷氧基酸的至少一种钾盐中的磷在0.6至1.4的范围内; (ii)将(i)中提供的液体进料流送入包含催化剂的环氧化反应器中,所述催化剂包含含锌的结构型MVVW的钛沸石,并使液体进料流在环氧化反应器中进行环氧化反应条件,得到反应混合物 包括环氧丙烷,乙腈,水,所述至少一种溶解的含磷酸的钾盐,任选的丙烯,以及任选的丙烷; (iii)从环氧化反应器中除去流出物流,所述流出物流包含环氧丙烷,乙腈,水,所述至少一种溶解的含磷酸的钾盐,任选的丙烯和任选的丙烷的至少一部分。
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公开(公告)号:US20240408585A1
公开(公告)日:2024-12-12
申请号:US18274042
申请日:2022-01-25
Applicant: BASF SE
Inventor: Andrey KARPOV , Christian ALMER , Christian WALSDORFF , Andreas LEHR , Michael NIKOLAY , Christian BARTOSCH , Mauricio GROBYS
IPC: B01J27/055 , B01J21/04 , B01J23/68 , B01J35/61 , B01J35/63 , B01J37/02 , B01J37/08 , C07D301/10
Abstract: An epoxidation catalyst comprising silver, cesium, rhenium and tungsten deposited on an alumina support, wherein the catalyst comprises 20 to 50 wt.-% of silver, relative to the weight of the catalyst, an amount of cesium Ccs of at least 7.5 mmol per kg of catalyst, and an amount of rhenium CR6 and an amount of tungsten Cw so as to meet the following requirements: CRe≥6.7 mmol per kg of catalyst; and CRe+(2χcw)≥13.2 mmol per kg of catalyst. The epoxidation catalyst allows for a more efficient conversion of ethylene oxide by gas-phase oxidation of ethylene, particularly displaying high selectivity and high activity. The invention also relates to a process for preparing an epoxidation catalyst as defined in above, comprising i) impregnating an alumina support with a silver impregnation solution; and ii) subjecting the impregnated refractory support to a calcination process; wherein steps i) and ii) are optionally repeated, and at least one silver impregnation solution comprises rhenium, tungsten and cesium. The invention moreover relates to a process for producing ethylene oxide by gas-phase oxidation of ethylene, comprising reacting ethylene and oxygen in the presence of an epoxidation catalyst according to any one of the preceding claims.
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公开(公告)号:US20210379569A1
公开(公告)日:2021-12-09
申请号:US17285799
申请日:2019-09-19
Applicant: BASF SE
Inventor: Andrey KARPOV , Marco Oskar KENNEMA , Nicolas DUYCKAERTS , Christian WALSDORFF , Christian BARTOSCH , Juergen ZUEHLKE , Miguel Angel
Abstract: A shaped catalyst body for producing ethylene oxide by gas-phase oxidation of ethylene, comprising silver deposited on a porous refractory support, the shaped catalyst body having a first face side surface, a second face side surface and a circumferential surface, characterized by a content of at least 20 wt.-% of silver, relative to the total weight of the shaped catalyst body; a multilobe structure; a plurality of passageways extending from the first face side surface to the second face side surface, outer passageways being arranged around a central passageway with one outer passageway being assigned to each lobe, wherein neighboring outer passageways are arranged essentially equidistantly to each other and the outer passageways are arranged essentially equidistantly to the central passageway; a minimum wall thickness A between two neighboring passageways in the range of 0.6 to 1.3 mm; a minimum wall thickness B between each outer passageway and the circumferential surface in the range of 1.1 to 1.8 mm; and a BET surface area in the range of 1.6 to 3.0 m2/g. The shaped catalyst bodies allow for a favorable balance between mechanical stability, pressure drop and selectivity. The invention also relates to a process for producing ethylene oxide by gas-phase oxidation of ethylene, comprising reacting ethylene and oxygen in the presence of a shaped catalyst body as defined above. The invention further relates to a process for preparing a shaped catalyst body as above, comprising i) impregnating a refractory support having a BET surface area in the range of 1.4 to 2.5 m2/g with a silver impregnation solution; and ii) subjecting the impregnated refractory support to a calcination process; wherein steps i) and ii) are optionally repeated.
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公开(公告)号:US20210283583A1
公开(公告)日:2021-09-16
申请号:US16323828
申请日:2017-08-08
Applicant: BASF SE
Inventor: ANDREY KARPOV , Michael KRAEMER , Marco BOSCH , Christian BARTOSCH , Juergen ZUEHLKE , Carlos LIZANDARA PUEYO , Guido WASSERSCHAFF
Abstract: The present invention is directed to a shaped catalyst body for preparing ethylene oxide, which comprises at least silver, cesium and rhenium applied to an alumina support, wherein the alumina support comprises Si, Ca, and Mg in a defined amount. Furthermore, the present invention is directed to a process for preparing the catalyst according to the present invention and process for preparing ethylene oxide by gas-phase oxidation of ethylene by means of oxygen in the presence of a shaped catalyst body according to the present invention.
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公开(公告)号:US20210046459A1
公开(公告)日:2021-02-18
申请号:US16968542
申请日:2019-02-06
Applicant: BASF SE
Inventor: Andrey KARPOV , Christian WALSDORFF , Michael KRAEMER , Armin LANGE DE OLIVEIRA , Gerhard KRENNRICH , Christian BARTOSCH , Juergen ZUEHLKE
Abstract: The present invention provides a catalyst effective in the oxidative conversion of ethylene to ethylene oxide, comprising an alumina support and 20 to 45%by weight of the catalyst, of silver applied to the support, the catalyst meeting the following limitations (i) to (v): (i) an amount of cesium c(Cs) in mmol per Kg of catalyst of at least 2; (ii) an amount of rhenium c(Re) in mmol per Kg of catalyst of at least 3.0; (iii) an amount of tungsten c(W) in mmol per Kg of catalyst of at least 1.6; (iv) a silicon to alkaline earth metal molar ratio x of not higher than 1.80; (v) c(Cs)−c(Re)−c(W)≤4·x−0.5.
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公开(公告)号:US20210039074A1
公开(公告)日:2021-02-11
申请号:US16968548
申请日:2019-02-06
Applicant: BASF SE
Inventor: Andrey KARPOV , Andreas LEHR , Daniela RIECK , Holger BORCHERT , Tobias WEINLAND , Marco BOSCH , Christian WALSDORFF , Christian BARTOSCH , Juergen ZUEHLKE
Abstract: A method for preparing a silver impregnation solution comprises (a) charging a neutralization reactor R1 with an aqueous organic amine; (b) adding oxalic acid powder through a first feeding conduit to the neutralization reactor R1 to obtain an aqueous oxalic acid-organic amine solution; (c) directing the aqueous oxalic acid-organic amine solution from the neutralization reactor to a complexation reactor R2; (d) adding particulate silver oxide through a second feeding conduit to the complexation reactor R2 to obtain a silver impregnation solution; and, optionally, (e) subjecting the silver impregnation solution to filtration. The silver impregnation solution is used for producing a catalyst effective in the oxidative conversion of ethylene to ethylene oxide. The method allows for the preparation of a silver impregnation solution in an efficient and occupationally and environmentally safe way. Security hazards which can occur when oxalic acid and silver oxide are added to an aqueous amine solution using the same powder feeding equipment or the same reactor are avoided.
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